Three-Dimensional Molecular Mapping of Ionic Liquids at Electrified Interfaces

被引:52
|
作者
Zhou, Shan [1 ,2 ]
Panse, Kaustubh S. [1 ,2 ]
Motevaselian, Mohammad Hossein [3 ]
Aluru, Narayana R. [3 ]
Zhang, Yingjie [1 ,2 ]
机构
[1] Univ Illinois, Dept Mat Sci & Engn, Urbana, IL 61801 USA
[2] Univ Illinois, Mat Res Lab, Urbana, IL 61801 USA
[3] Univ Illinois, Dept Mech Sci & Engn, Urbana, IL 61801 USA
基金
美国国家科学基金会;
关键词
electrochemical AFM; 3D-AFM; ionic liquid; electric double layer; solid-liquid interface; electrode-electrolyte interface; ATOMIC-FORCE MICROSCOPY; DOUBLE-LAYER; AQUEOUS-SOLUTIONS; FIELD PARAMETERS; WATER; ELECTROLYTE; DYNAMICS; TRANSITIONS; SCIENCE; CATIONS;
D O I
10.1021/acsnano.0c07957
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electric double layers (EDLs), occurring ubiquitously at solid-liquid interfaces, are critical for electrochemical energy conversion and storage processes such as capacitive charging and redox reactions. However, to date the molecular-scale structure of EDLs remains elusive. Here we report an advanced technique, electrochemical three-dimensional atomic force microscopy (EC-3D-AFM), and use it to directly image the molecular-scale EDL structure of an ionic liquid under different electrode potentials. We observe not only multiple discrete ionic layers in the EDL on a graphite electrode but also a quasi-periodic molecular density distribution within each layer. Furthermore, we find pronounced 3D reconfiguration of the EDL at different voltages, especially in the first layer. Combining the experimental results with molecular dynamics simulations, we find potential-dependent molecular redistribution and reorientation in the innermost EDL layer, both of which are critical to EDL capacitive charging. We expect this mechanistic understanding to have profound impacts on the rational design of electrode-electrolyte interfaces for energy conversion and storage.
引用
收藏
页码:17515 / 17523
页数:9
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